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充電された逆ミセルの酸プールにおける陽子輸送の高度な変化状態
Hongxia Hao1, Ellen M Adams2,3, Sarah Funke4
1Kenneth S. Pitzer Center for Theoretical Chemistry, Department of Chemistry, University of California, Berkeley, California94720, United States.
Journal of the American Chemical Society
|January 12, 2023
まとめ
充電された逆ミセル (RMs) での陽子輸送は著しく阻害されています. NaAOTやCTABrのような 充電された表面活性物質は 陽子のジャンプを阻害し 閉じ込められた酸のプール内の動態を遅らせます
科学分野:
- 物理化学
- コンピュータ化学
- 材料科学
背景:
- リバースミセル (RMs) は水溶液を閉じ込めるために使用される多用途のナノ構造体です.
- 閉じ込められた環境での陽子輸送を理解することは,触媒と生物学的プロセスにとって極めて重要です.
- RMの充電された表面活性物質は,閉じ込められた液体の性質を大幅に変化させることができます.
研究 の 目的:
- 充電された表面活性物質で反転ミセル (RMs) の陽子輸送のメカニズムを調査する.
- シミュレーション結果と実験用スペクトロスコピデータ (テラヘルツ吸収と介電リラクゼーション) を相関させる.
- 限られた酸性プール内の陽子の動力学における表面活性物質の電荷の役割を解明する.
主な方法:
- 反応力場シミュレーションは,陽子のダイナミクスをモデル化するために使用されました.
- 分析は,ナトリウムビス・エチルヘキシル硫酸塩 (NaAOT) とセチルトリメチルアモニウムブロミド (CTABr) のRM内の輸送機構に焦点を当てた.
- 非イオン型RMと実験用スペクトルシグネチャーとの比較.
主要な成果:
- 陽子ジャンプは,ナオットRMと非イオンRMに比べて抑制された.
- CTABr RMsでは,陽子輸送のためのGrotthussメカニズムが完全に抑制されました.
- 充電されたヘッドグループとカウンタリオンは,インターフェイスのイオン濃度を変化させ,RM内の有効pHを増加させた.
- コントリオン/結合塩基の近くの陽子の局所化は,EigenとZundelの構成を阻害し,局所振動のジャンプを好みました.
結論:
- 充電された表面活性物質は,反転ミセルのプロトン輸送を大幅に阻害します.
- 観測された遅いプロトンダイナミクスは,静電相互作用と局所的なpHの変化に起因する.
- 局所振動のジャンプが支配的になり,特にCTABr RMでは,陽子の滞在時間が延長されます.
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